Kinetic of adsorption and of photocatalytic degradation of phenylalanine effect of pH and light intensity

被引:36
作者
Elsellami, L. [1 ]
Vocanson, F. [2 ,3 ]
Dappozze, F. [1 ]
Puzenat, E. [1 ]
Paisse, O. [4 ]
Houas, A.
Guillard, C. [1 ]
机构
[1] Univ Lyon 1, CNRS, IRCELYON, UMR 5256, F-69626 Villeurbanne, France
[2] Univ St Etienne, F-42000 St Etienne, France
[3] Lab Hubert Curien, UMR 5516, F-42000 St Etienne, France
[4] CNRS, Serv Cent Anal, F-69390 Vernaison, France
关键词
Phenylalanine; Adsorption; Photocatalysis; Kinetic; By-products; pH; Radiant flux; AMINO-ACIDS; WATER; TIO2; MINERALIZATION;
D O I
10.1016/j.apcata.2010.03.054
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Phenylalanine (Phe) was chosen to study the TiO2 photocatalytic degradation of amino acids, which are at the origin of the formation of odorous compounds after chlorination. The photocatalytic degradation has been investigated in aqueous solutions containing TiO2 suspensions as photocatalyst, in order to assess the influence of various parameters, such as adsorption, initial concentration, pH and radiant flux on the photocatalytic process. Results showed no correlation between dark adsorption and photocatalytic degradation. A multilayer kinetic was observed in the dark with a monolayer corresponding to less that 1% of OH covered, whereas Langmuir-Hinshelwood model seems to modelize the photocatalytic disappearance of Phe. However, even if the form of the curve is similar to L-H model, the degradation of phenylalanine is not a kinetic of L-H as we could plan it by considering the adsorption of the phenylalanine in the dark. The study of the mineralization of carbon and nitrogen showed that nitrogen atoms were predominantly photoconverted into NH4+ and a total mineralization of nitrogen and carbon seems occur. The identification of the by-products by LC-MS reveal mono- and di-hydroxylation and nitrogen-carbon (N-C) cleavage. The effect of pH showed an increase of adsorption under acid pH but a decrease of disappearance rate. The more efficient degradation was found at basic pH. The evolution of hydroxylated compounds of phenylalanine as a function of conversion revealed the presence of more hydroxylated compounds at natural pH and at basic pH compared to acid pH suggesting a modification of mechanism with solution pH. The effect of the radiant flux evaluated under different initial concentration of phenylalanine allowed us to determine that k increases by increasing the radiant flux, whereas K decreases or remains constant from about a value of 3.5 mW/cm(2). The disappearance rate as a function of radiant flux has been showed to reach a maximal value corresponding to a maximal quantum yield of 1.6%. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:142 / 148
页数:7
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